Novel hierarchical ZnO nanoarchitectures, such as microtrepangs, microbelts, nanoflowers, nanocombs, nanowheels, and nanofans assembled by ZnO nanocones, nanobowling pins, nanobottles, nanoarrows, and nanonails, have had their growth controlled by the thermal evaporation of Zn and a mixture of In and In2S3. Both the morphologies of the products and their construction units could be efficiently controlled by simple adjustment of the weight ratio of In/In2S3. The phase structure, morphologies, and photoluminescence properties of the ZnO products were investigated by X-ray diffraction, scanning electron microscopy, high-resolution transmission electron microscopy, and photoluminescence spectroscopy. These novel hierarchical ZnO nanoarchitectures may be attractive building blocks for creating optical or other nanodevices.